Oxygen Evolution/Reduction Reaction Catalysts: From In Situ Monitoring and Reaction Mechanisms to Rational Design

Chemical Reviews, Год журнала: 2023, Номер 123(9), С. 6257 - 6358

Опубликована: Март 21, 2023

The oxygen evolution reaction (OER) and reduction (ORR) are core steps of various energy conversion storage systems. However, their sluggish kinetics, i.e., the demanding multielectron transfer processes, still render OER/ORR catalysts less efficient for practical applications. Moreover, complexity catalyst–electrolyte interface makes a comprehensive understanding intrinsic mechanisms challenging. Fortunately, recent advances in situ/operando characterization techniques have facilitated kinetic monitoring under conditions. Here we provide selected highlights mechanistic studies with main emphasis placed on heterogeneous systems (primarily discussing first-row transition metals which operate basic conditions), followed by brief outlook molecular catalysts. Key sections this review focused determination true active species, identification sites, reactive intermediates. For in-depth insights into above factors, short overview metrics accurate characterizations is provided. A combination obtained time-resolved information reliable activity data will then guide rational design new Strategies such as optimizing restructuring process well overcoming adsorption-energy scaling relations be discussed. Finally, pending current challenges prospects toward development homogeneous presented.

Язык: Английский

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S‐Scheme Co₉S₈@Cd_0.8Zn_0.2S‐DETA Hierarchical Nanocages Bearing Organic CO₂ Activators for Photocatalytic Syngas Production

Advanced Energy Materials, Год журнала: 2023, Номер 13(15)

Опубликована: Март 1, 2023

Abstract Delicate modulations of CO 2 activation and charge carrier separation/migration are challenging, yet imperative to augment photoreduction efficiency. Herein, by supporting diethylenetriamine (DETA)‐functionalized Cd 0.8 Zn 0.2 S nanowires on the exterior surface hollow Co 9 8 polyhedrons, hierarchical @Cd S‐DETA nanocages fabricated as an S‐scheme photocatalyst for reducing protons produce syngas (CO H ). The amine groups strengthen adsorption , while “nanowire‐on‐nanocage” heterostructure with interface boosts separation transfer photoinduced charges. Employing Co(bpy) 3 2+ a cocatalyst, optimal effectively produces in rates 70.6 18.6 µmol h −1 (i.e., 4673 1240 g ), respectively, affording apparent quantum efficiency 9.45% at 420 nm, which is highest value under comparable conditions. Ultraviolet photoelectron spectroscopy, Kelvin probe, electron spin resonance confirm S‐schematic charge‐transfer process photocatalyst. key COOH * species responsible ‐to‐CO reduction detected in‐situ diffuse reflectance infrared Fourier transform spectroscopy endorsed density functional theory calculations, thus possible mechanism proposed.

Язык: Английский

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Robust and durable liquid-repellent surfaces

Chemical Society Reviews, Год журнала: 2022, Номер 51(20), С. 8476 - 8583

Опубликована: Янв. 1, 2022

Liquid-repellent surfaces, such as superhydrophobic superoleophobic and slippery liquid-infused have drawn keen research interest from the communities engaged in chemical synthesis, interfacial chemistry, surface engineering, bionic manufacturing micro-nano machining. This is due to their great potential applications liquid-proofing, self-cleaning, resistance, anti-icing, water/oil remediation, biomedicine, etc. However, poor robustness durability that notably hinders real-world of surfaces remains Achilles heel. The past few years witnessed rapidly increasing publications address liquid-repellent many breakthroughs been achieved. review provides an overview recent progress made towards robust durable surfaces. First, we discuss wetting solid its generally-adopted characterisation methods, introduce typical Second, focus on various evaluation methods Third, advances design fabrication are reviewed detail. Fourth, present where these employed fields like biology daily life. Finally, possible perspectives By presenting state-of-the-art this significant fast-developing area, believe will inspire multidisciplinary scientific industrial circles develop novel can meet requirements applications.

Язык: Английский

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Hydrogen society: from present to future

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4926 - 4943

Опубликована: Янв. 1, 2023

Systematic insights into the recent attainments, limitations, and future directions of hydrogen production, storage, delivery, usage are provided, aiming at offering critical guidance for establishment a society.

Язык: Английский

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Dual interfacial engineering of a Chevrel phase electrode material for stable hydrogen evolution at 2500 mA cm−2

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Окт. 26, 2022

Constructing stable electrodes which function over long timescales at large current density is essential for the industrial realization and implementation of water electrolysis. However, rapid gas bubble detachment usually results in peeling-off electrocatalysts performance degradation, especially term operations. Here we construct a mechanically-stable, all-metal, highly active CuMo6S8/Cu electrode by in-situ reaction between MoS2 Cu. The Chevrel phase exhibits strong binding electrocatalyst-support interface with weak adhesion electrocatalyst-bubble interface, addition to fast hydrogen evolution charge transfer kinetics. These features facilitate achievement 2500 mA cm-2 small overpotential 334 mV operate stably 100 h. In-situ total internal reflection imaging micrometer level mechanical tests disclose relationships two interfacial forces electrocatalysts. This dual engineering strategy can be extended high-performance other gas-involving reactions.

Язык: Английский

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Identifying a Universal Activity Descriptor and a Unifying Mechanism Concept on Perovskite Oxides for Green Hydrogen Production

Advanced Materials, Год журнала: 2023, Номер 35(44)

Опубликована: Июль 15, 2023

Producing indispensable hydrogen and oxygen for social development via water electrolysis shows more prospects than other technologies. Although electrocatalysts have been explored centuries, a universal activity descriptor both hydrogen-evolution reaction (HER) oxygen-evolution (OER) is not yet developed. Moreover, unifying concept established to simultaneously understand HER/OER mechanisms. Here, the relationships between activities in three common electrolytes over ten representative material properties on 12 3d-metal-based model oxides are rationally bridged through statistical methodologies. The orbital charge-transfer energy (Δ) can serve as an ideal descriptor, where neither too large nor small Δ (≈1 eV) with optimal electron-cloud density around Fermi level affords best activities, fulfilling Sabatier's principle. Systematic experiments computations unravel that pristine oxide ≈ 1 eV possesses metal-like high-valence configurations active lattice-oxygen sites help adsorb key protons HER induce participation OER, respectively. After reactions, partially generated metals hydroxides OER dominate proton adsorption couple activation, These be successfully rationalized by theory. This work provides foundation of rational design mechanism understanding many potential applications.

Язык: Английский

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Hierarchically Ordered Macro–Mesoporous Electrocatalyst with Hydrophilic Surface for Efficient Oxygen Reduction Reaction

Advanced Materials, Год журнала: 2023, Номер 35(30)

Опубликована: Апрель 18, 2023

Metal-organic frameworks (MOFs) offer versatile templates/precursors to prepare supported metal catalysts. However, the afforded catalysts usually exhibit microporous structures and unsuitable wettability, which will restrict accessibility of active sites in liquid-phase reactions. Herein, an etching-functionalization strategy is developed for construction a tannic-acid-functionalized MOF with unique hollow-wall 3D-ordered macroporous (H-3DOM) structure. The functional can be further employed as ideal precursor synthesis cobalt on oxygen/nitrogen-co-doped carbon composites H-3DOM structures, hydrophilic surface. structure improve external surface area maximize exposure sites. Moreover, oxygen-containing groups enhance wettability guarantee more electrochemically accessible aqueous electrolyte. Benefitting from these outstanding characteristics, H-3DOM-Co/ONC exhibits high electrocatalytic activity oxygen reduction reaction, superior its counterparts without hierarchically ordered functionalization.

Язык: Английский

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Strategies for Sustainable Production of Hydrogen Peroxide via Oxygen Reduction Reaction: From Catalyst Design to Device Setup

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Май 9, 2023

Abstract An environmentally benign, sustainable, and cost-effective supply of H 2 O as a rapidly expanding consumption raw material is highly desired for chemical industries, medical treatment, household disinfection. The electrocatalytic production route via electrochemical oxygen reduction reaction (ORR) offers sustainable avenue the on-site from O. most crucial innovative part such technology lies in availability suitable electrocatalysts that promote two-electron (2e – ) ORR. In recent years, tremendous progress has been achieved designing efficient, robust, catalyst materials, including noble metals their alloys, metal-free carbon-based single-atom catalysts, molecular catalysts. Meanwhile, cell designs have significantly advanced applications at industrial level. This review summarizes fundamental basics advances 2e -ORR, design, mechanistic explorations, theoretical computations, experimental evaluations, designs. Perspectives on addressing remaining challenges are also presented with an emphasis large-scale synthesis route.

Язык: Английский

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Electrosynthesis of hydrogen peroxide via two-electron oxygen reduction reaction: A critical review focus on hydrophilicity/hydrophobicity of carbonaceous electrode

Chemical Engineering Journal, Год журнала: 2022, Номер 450, С. 138246 - 138246

Опубликована: Июль 22, 2022

Язык: Английский

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An anti-electrowetting carbon film electrode with self-sustained aeration for industrial H₂O₂ electrosynthesis

Energy & Environmental Science, Год журнала: 2023, Номер 17(2), С. 655 - 667

Опубликована: Ноя. 28, 2023

A novel concept of an anti-electrowetting carbon film electrode with self-sustained aeration was devised and demonstrated to develop next-generation cheap scalable metal-free electrodes for industry-scale H 2 O electrosynthesis.

Язык: Английский

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